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A nonlinear conjugate gradient optimization scheme is used to obtain excitation energies within the random phase approximation (RPA). The solutions to the RPA eigenvalue equation are located through a variational characterization using a modified Thouless functional, which is based upon an asymmetric Rayleigh quotient, in an orthogonalized atomic orbital(More)
Four different numerical algorithms suitable for a linear scaling implementation of time-dependent Hartree-Fock and Kohn-Sham self-consistent field theories are examined. We compare the performance of modified Lanczos, Arooldi, Davidson, and Rayleigh quotient iterative procedures to solve the random-phase approximation (RPA) (non-Hermitian) and Tamm-Dancoff(More)
The Condon approximation is widely applied in molecular and condensed matter spectroscopy and states that electronic transition dipoles are independent of nuclear positions. This approximation is related to the Franck-Condon principle, which in its simplest form holds that electronic transitions are instantaneous on the time scale of nuclear motion. The(More)
We employ scanning tunneling microscopy (STM) to reveal the structure of DNA-carbon nanotube complexes with unprecedented spatial resolution and compare our experimental results to molecular dynamics simulations. STM images show strands of DNA wrapping around (6,5) nanotubes at approximately 63 degrees angle with a coiling period of 3.3 nm, in agreement(More)
State-of-the-art photovoltaics use high-purity, large-area, wafer-scale single-crystalline semiconductors grown by sophisticated, high-temperature crystal growth processes. We demonstrate a solution-based hot-casting technique to grow continuous, pinhole-free thin films of organometallic perovskites with millimeter-scale crystalline grains. We fabricated(More)
We report on the dynamics of resonant energy transfer in monodisperse, mixed-size, and energy-gradient (layered) assemblies of CdSe nanocrystal quantum dots. Time-resolved and spectrally resolved photoluminescence directly reveals the energy-dependent transfer rate of excitons from smaller to larger dots via electrostatic coupling. The data show a rapid(More)
We study theoretically two electron-hole pair states (biexcitons) in core/shell hetero-nanocrystals with type II alignment of energy states, which promotes spatial separation of electrons and holes. To describe Coulomb interactions in these structures, we apply first-order perturbation theory, in which we use an explicit form of the Coulomb-coupling(More)
We investigate the impact of ligands on the morphology, electronic structure, and optical response of the Cd(33)Se(33) cluster, which overlaps in size with the smallest synthesized CdSe nanocrystal quantum dots (QDs). Our density functional theory calculations demonstrate significant surface reorganization for both the bare cluster and the cluster capped(More)
We report a two-step synthesis of highly luminescent CdS/ZnSe core/shell nanocrystals (emission quantum yields up to 50%) that can produce efficient spatial separation of electrons and holes between the core and the shell (type-II localization regime). Our synthesis involves fabrication of cubic-singony CdS core particles that are subsequently overcoated(More)